Integration of theory, simulation, artificial intelligence and virtual reality: a four-pillar approach for reconciling accuracy and interpretability in computational spectroscopy
Modern multireference methods and their application in transition metal chemistry
Homogeneous nucleation of sheared liquids: advances and insights from simulations and theory
Computational approaches for analyzing the homogeneous nucleation of sheared simple liquids are reviewed. We examine underlying mechanisms and effects of flow. The experimental scope and sheared nucleation of polymers and glasses are also covered.
Picture-change correction in relativistic density functional theory
The picture-change-corrected two-component relativistic density functional theory (PCC-2c-DFT) adopts the correctly transformed electron density, exchange–correlation potential, and two-electron operator.
Bicolour fluorescent molecular sensors for cations: design and experimental validation
In this perspective the main design criteria of fluorescent bicolour sensors for metallic cations are presented, as well as selected examples illustrating the high efficiency and versatility of this technique.
A review on two-dimensional materials for chemiresistive- and FET-type gas sensors
The recent development of 2D material-based chemiresistive- and FET-type gas sensors as well as their future directions are comprehensively presented.
Computational modelling of Pd-catalysed alkoxycarbonylation of alkenes and alkynes
How theory and computation can afford mechanistic insights into important reactions in homogeneous catalysis.
Electron spin dynamics in excited state photochemistry: recent development in the study of intersystem crossing and charge transfer in organic compounds
Recent developments of electron spin dynamics in organic molecular systems studied by time-resolved electron paramagnetic spectroscopy are summarized.
An overview of hydroxy-based polyanionic cathode insertion materials for metal-ion batteries
The inspiration and challenge for through-space charge transfer architecture: from thermally activated delayed fluorescence to non-linear optical properties
In this perspective, we review the TADF properties of D–π–A molecules with through-space charge transfer architecture with focus on their regulating effects toward NLO responses.
The π-hole revisited
Two views of the computed electrostatic potential on the 0.001 au surface of 2,4,6-trifluoro-1,3,5-triazine. Red is the most positive color range, while blue is the most negative.
Phenothiazine functional materials for organic optoelectronic applications
This prospective provides a brief overview of the working principles of various optoelectronic devices and the structure–property relationships in phenothiazine.
Implications of relaxation dynamics of collapsed conjugated polymeric nanoparticles for light-harvesting applications
The mechanism of the formation of nanoparticles (collapsed state) from the extended state of polymers and their ultrafast excited state relaxation dynamics are illustrated.
Molecular modelling of compounds used for corrosion inhibition studies: a review
This perspective review features, among others, the use of DFT, QSAR modeling, artificial neural network (ANN) modeling, molecular dynamics simulations and Monte Carlo simulations in modelling organic corrosion inhibitors. It is a compendium of studies on the subject.
Environment-friendly Cu-based Compounds Thin Film Solar Cells: Materials, Devices and Charge Carrier Dynamics
Thermal and Photo Stability of All Inorganic Lead Halide Perovskite Nanocrystals
Energy storage electrochromic devices in the era of intelligent automation
A catalog summary and capacity comparison of ECESDs.
Progress in phase-sensitive sum frequency generation spectroscopy
Representative methods of surface-selective phase-sensitive sum frequency generation spectroscopy are reviewed in terms of interferometer implementation for optical heterodyne detection.
Possible effects of fluxionality of a cavitand on its catalytic activity through confinement
Atomic clusters and cavitands facilitate important chemical phenomena like hydrogen storage, catalysis, bond activation, etc. Additional fluxional behaviour along with the effects of confinement may exhibit dramatic changes in the reactions within.
Review on physical impedance models in modern battery research
An overview of modern physical impedance models in battery research is provided with selected examples dealing with traditional, aqueous, and all-solid-state systems.
Recent advances on enhancing the multicarbon selectivity of nanostructured Cu-based catalysts
This article reviews the recent progress and emerging strategies for achieving the selective conversion of CO2 to multicarbon reaction products on Cu-based catalysts.
Weak covalent interactions and anionic charge-sharing polymerisation in cluster environments
How solvation obstructs charge sharing and limits the size of covalently bound core anions in clusters.
Perspective on computational reaction prediction using machine learning methods in heterogeneous catalysis
Machine learning algorithms can facilitate the reaction prediction in heterogeneous catalysis.
Design and perspective of amorphous metal nanoparticles from laser synthesis and processing
Pulsed laser strategies (i.e. pulsed laser ablation and fragmentation in liquid) have been reviewed with a focus on the synthesis and processing of amorphous metal nanoparticles. The possible formation criteria and mechanism have been discussed.
Improved insights in time-resolved photoelectron imaging
We review new light source developments and data analysis considerations relevant to the time-resolved photoelectron imaging technique. Case studies illustrate how these themes may enhance understanding in studies of excited state molecular dynamics.
Ordered mesoporous metal oxides for electrochemical applications: correlation between structure, electrical properties and device performance
In this Perspective, the authors review the interplay between structure and charge-transport properties of mesoporous metal oxides, with an emphasis on applications in electrochemical energy storage, catalysis and gas sensing.
This article reviews the scope of inorganic cluster compounds measured in single-molecule junctions. The article explores how the structure and bonding of inorganic clusters give rise to specific quantum transport phenomena in molecular junctions.
Transport of charge carriers and optoelectronic applications of highly ordered metal phthalocyanine heterojunction thin films
A review on transport of charge carriers of highly ordered metal phthalocyanine heterojunction thin films fabricated by the weak epitaxy growth method, including various characterization techniques and optoelectronic applications is presented.
Computational approaches to dissociative chemisorption on metals: towards chemical accuracy
The theoretical description of dissociative chemisorption of isolated molecules on metal surfaces is discussed. Emphasis is put on methods that deliver chemical accuracy for the dissociative chemisorption probability S0, so that Δ ≤ 1 kcal mol−1.
Substance and shadow of formamidinium lead triiodide based solar cells
We shed light on the compositional, surface engineering and crystallization kinetics manipulations for FAPbI3 followed by a proposition for unified testing protocols in order to scale-up the solar cells from the lab to the market.
Lithium ion battery degradation: what you need to know
The expansion of lithium-ion batteries from consumer electronics to larger-scale transport and energy storage applications has made understanding the many mechanisms responsible for battery degradation increasingly important.
Ultrafast photoinduced dynamics in Prussian blue analogues
A review on ultrafast photoinduced processes in molecule-based magnets with an emphasis on Prussian blue analogues.
Defect-related dynamics of photoexcited carriers in 2D transition metal dichalcogenides
Defects participate various relaxation mechanisms and alter the trace and time scale of the decay process in two-dimensional (2D) transition metal dichalcogenides (TMDs).
First-principles calculations of hybrid inorganic–organic interfaces: from state-of-the-art to best practice
This work highlights the challenges and problems when modelling inorganic–organic interfaces and provides practical tips and suggestions for efficient calculations.
Quantum and semiclassical dynamical studies of nonadiabatic processes in solution: achievements and perspectives
We concisely review the most used methodological approaches to model nonadiabatic dynamics in isotropic solutions and their applications.
Material properties particularly suited to be measured with helium scattering: selected examples from 2D materials, van der Waals heterostructures, glassy materials, catalytic substrates, topological insulators and superconducting radio frequency materials
This paper presents material properties particularly suited to be measured with helium scattering techniques. Below a specific science case example illustrating the measurement of the electron–phonon coupling constant λ on a topological insulator surface.
Grazing incidence fast atom diffraction, similarities and differences with thermal energy atom scattering (TEAS)
In the elastic regime, GIFAD is equivalent to TEAS with an effective energy E⊥ between 1 meV and 1 eV providing a high sensitivity to topology and to attractive forces. The inelastic regime merges to the classical limit and is still in development.
Atom-surface van der Waals potentials of topological insulators and semimetals from scattering measurements
Gas-surface scattering experiments yield high accuracy interaction potentials in the van der Waals regime. A perspective overview for topological semimetals & insulators is provided and the importance for benchmarking ab initio calculations outlined.
The electron–phonon coupling constant for single-layer graphene on metal substrates determined from He atom scattering
A theory, previously formulated for conducting surfaces, is extended to extract the electron-phonon coupling strength λ for graphene supported on metal substrates from the thermal attenuation (Debye–Waller factor) of helium scattering reflectivity.
Time-dependent quantum mechanical wave packet dynamics
Starting from a model study of the collinear (H, H2) exchange reaction in 1959, the time-dependent quantum mechanical wave packet (TDQMWP) method has come a long way in dealing with systems as large as Cl + CH4.
Metal clusters synthesized in helium droplets: structure and dynamics from experiment and theory
In this Perspective we present the state of the art of creating mixed metal clusters in the superfluid droplet environment and their investigation through a successful interplay between experimental characterization and theoretical modelling.
Chemical reactions on surfaces for applications in catalysis, gas sensing, adsorption-assisted desalination and Li-ion batteries: opportunities and challenges for surface science
Chemical reactions on surfaces of innovative materials have direct implications in application fields, such as catalysis, batteries, gas sensing and desalination.
Targeted modifications in ionic liquids – from understanding to design
The large number of possible ionic liquids makes fully empirical design virtually impossible. In this work, we show how targeted modifications can be and have been used to find the relevant structural features that define the properties of ionic liquids.
Understanding the structure, bonding and reactions of nanocrystalline semiconductors: a novel high-resolution instrumental method of solid-state synchronous luminescence spectroscopy
Solid-state synchronous luminescence spectroscopy (SS-SLS) is a novel high-resolution method to study the absorption and emission of light, electronic structure, and reactions of nanocrystalline semiconductors.
Origins and properties of the tetrel bond
Tetrel bonds are dependent on modification of electron density and electrostatic potential caused by a substituent.
O–H stretching frequency red shifts do not correlate with the dissociation energies in the dimethylether and dimethylsulfide complexes of phenol derivatives
In the complexes of dimethylether and dimethylsulfide with various phenol derivatives the conventional Badger–Bauer rule is violated, i.e., the red shift in the OH stretching frequency does not correlate with the H-bonding strength.
An analysis of electrophilic aromatic substitution: a “complex approach”
A bigger mechanistic picture of electrophilic aromatic substitution (EAS) is summarized and important “missing” postulates in EAS are unified.
Microfluidic technologies for the synthesis and manipulation of biomimetic membranous nano-assemblies
A mini-review of microfluidic technologies for the generation and manipulation of biomimetic nano-assemblies, including perspectives for future research directions.
Pickup and reactions of molecules on clusters relevant for atmospheric and interstellar processes
In this perspective, we review experiments with molecules picked up on clusters in molecular beams with the focus on the processes in atmospheric and interstellar chemistry.
Recent progress in approximate quantum dynamics methods for the study of proton-coupled electron transfer reactions
We provide a detailed theoretical background and methodological perspective for the application of recently-developed quantum dynamics methods to the study of PCET, including discussion of several recent demonstrations.
Towards peptide-based tunable multistate memristive materials
Development of new memristive hardware is a technological requirement towards widespread neuromorphic computing. Biomolecules can help.
Perspective on multi-scale simulation of thermal transport in solids and interfaces
Phonon-mediated thermal transport is inherently multi-scale. The nature of multi-scale thermal transport is that there are different heat transfer physics across different length scales with strong entanglement and interaction with each other.
Recent progress in the development of thermal interface materials: a review
Recent progress in the development of thermal interface materials.
Viscosity models for ionic liquids and their mixtures
Review of principles and limitations of viscosity models for ionic liquids and their mixtures focusing on the use of inappropriate mixing rules for molten salts.
Confronting FCP structure with ultrafast spectroscopy data: evidence for structural variations
In this Perspective, we demonstrate that the published FCP structures are not entirely consistent with 2D spectroscopy results for Cyclotella meneghiniana. To remedy this issue, we propose pigment arrangement in the trimeric FCP for this species.
Recent advances in atomic molecular dynamics simulation of intrinsically disordered proteins
Atomic molecular dynamics simulation provides the most detailed description of intrinsically disordered proteins (IDPs).
Deep eutectic solvents as non-traditionally multifunctional media for the desulfurization process of fuel oil
This review summarizes the physicochemical properties of deep eutectic solvents (DESs) and their applications for the desulfurization processes of fuel oil. Moreover, current challenges and future opportunity are discussed.
Effects of ion migration and improvement strategies for the operational stability of perovskite solar cells
The fundamental factor (ion migration) affecting the stability of perovskite solar cells and improvement strategies have been reviewed.
Dielectric confinement for designing compositions and optoelectronic properties of 2D layered hybrid perovskites
The possibility of using nanoscale dielectric contrast for designing 2D layered halide perovskite compositions for optoelectronic applications is discussed.
Ultrafast processes: coordination chemistry and quantum theory
The correlation between electronic densities and active molecular vibrations drives the spin–vibronic mechanism of ultrafast decays in coordination chemistry.
Thermal enhancement of upconversion emission in nanocrystals: a comprehensive summary
Thermal enhancement of upconversion luminescence in lanthanide-doped nanocrystals are summarized and the enhancement mechanism is discussed in detail with a fresh perspective.
Behind the scenes of spin-forbidden decay pathways in transition metal complexes
Understanding the microscopic origin of spin-forbidden radiative and non-radiative photophysics of transition metal complexes with reference to spin–orbit coupling.
About this collection
Welcome to our online collection of PCCP Perspective articles. Here we feature PCCP Perspective articles published in 2021.
Perspectives are high profile articles that present an authoritative state-of-the-art account of the selected research field. PCCP Perspectives take a wide variety of forms including personal accounts of research, critical analyses of topics of current interest and essential introductions to a field.
Congratulations to all the authors whose articles are featured and we hope readers enjoy this collection.